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Vladislav Kataev

Publications and source records attributed to Vladislav Kataev.

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Magnetic anisotropy in the near-stoichiometric van der Waals ferromagnet Fe$_3$GeTe$_2$

Quasi-two-dimensional (2D) van der Waals (vdW) ferromagnets such as the series Fe$_{3-x}$GeTe$_2$, with a relatively high Curie temperature and robust metallicity, offer an ideal platform for investigating itinerant magnetism in reduced dimensions. Here, we present a comprehensive electron spin resonance (ESR) investigation of single-crystalline almost-stoichiometric Fe$_{3.03 \pm 0.03}$GeTe$_{2}$ across wide ranges of frequencies, temperatures, and magnetic fields to gain quantitative insights into its magnetic anisotropy and spin dynamics. Frequency-dependent ESR measurements establish Fe$_{3}$GeTe$_{2}$ as an easy-axis ferromagnet. Temperature-dependent high-field ESR reveals a large internal field that gradually decreases at higher temperatures. Remarkably, this internal field persists even above $T_\mathrm{C}$, evidencing short-range spin correlations in Fe$_{3}$GeTe$_{2}$. Analysis of spin-wave modes yields a strong uniaxial magnetocrystalline anisotropy $K_{\text{int}} \approx - 5 \times 10^6$ erg cm$^{-3}$ at 3 K and a large magnon gap $\Delta(3 \mathrm{K})$ $\approx$ 87.8 $\pm$ 13.7 GHz ($\approx$ 0.363 $\pm$ 0.057 meV). Our study highlights that small variations in Fe content in Fe$_{3}$GeTe$_{2}$ lead to substantial changes in the magnon gap at low temperatures, indicating the extreme sensitivity of spin dynamics to the chemical composition. These results establish Fe$_{3}$GeTe$_{2}$ as a model vdW ferromagnet for exploring tunable anisotropies and magnon excitations in metallic 2D magnets.

cond-mat.str-el

Magnetic-field tuning of the spin dynamics in the quasi-2D van der Waals antiferromagnet CuCrP$_{2}$S$_{6}$

The use of antiferromagnets in magnetoelectronic devices as counterparts of ferromagnets is a new, rapidly developing trend in spintronics that leverages antiferromagnetic (AFM) magnons for transmitting of spin currents. Van der Waals (vdW) antiferromagnets are particularly attractive in this respect as they possess tunable magnetic properties and can be easily integrated into spintronic devices. In this work we use electron spin resonance (ESR) spectroscopy to assess the potential of the vdW AFM compound CuCrP$_{2}$S$_{6}$ for magnonic applications by exploring the magnetic field ($H$) dependence of the spectrum of magnon excitations below its AFM ordering temperature $T_{\rm N} \approx 30$ K and the correlated spin dynamics above $T_{\rm N}$. ESR reveals prominent ferromagnetic (FM) spin correlations that persist far above $T_{\rm N}$ suggesting an intrinsically two-dimensional character of the spin dynamics in CuCrP$_{2}$S$_{6}$. Most interestingly, at $T < T_{\rm N}$, CuCrP$_{2}$S$_{6}$ features two non-degenerate, i.e., distinct in energy AFM magnon modes at $H = 0$ which can be tuned to the FM type of collective spin excitations with increasing $H$. These remarkable properties are favorable for the induction and control of unidirectional spin current in CuCrP$_{2}$S$_{6}$ and suggest it as a new functional material for magnetoelectronics.

cond-mat.str-el

Disentangling the unusual magnetic anisotropy of the near-room-temperature ferromagnet Fe$_{4}$GeTe$_{2}$

In the quest for two-dimensional conducting materials with high ferromagnetic ordering temperature the new family of the layered Fe$_{n}$GeTe$_{2}$ compounds, especially the near-room-temperature ferromagnet Fe$_{4}$GeTe$_{2}$, receives a significant attention. Fe$_{4}$GeTe$_{2}$ features a peculiar spin reorientation transition at $T_\mathrm{SR} \sim 110$ K suggesting a non-trivial temperature evolution of the magnetic anisotropy (MA) - one of the main contributors to the stabilization of the magnetic order in the low-D systems. An electron spin resonance (ESR) spectroscopic study reported here provides quantitative insights into the unusual magnetic anisotropy of Fe$_{4}$GeTe$_{2}$. At high temperatures the total MA is mostly given by the demagnetization effect with a small contribution of the counteracting intrinsic magnetic anisotropy of an easy-axis type, whose growth below a characteristic temperature $T_{\rm shape} \sim 150$ K renders the sample seemingly isotropic at $T_\mathrm{SR}$. Below one further temperature $T_{\rm d} \sim 50$ K the intrinsic MA becomes even more complex. Importantly, all the characteristic temperatures found in the ESR experiment match those observed in transport measurements, suggesting an inherent coupling between magnetic and electronic degrees of freedom in Fe$_{4}$GeTe$_{2}$. This finding together with the observed signatures of the intrinsic two-dimensionality should facilitate optimization routes for the use of Fe$_{4}$GeTe$_{2}$ in the magneto-electronic devices, potentially even in the monolayer limit.

cond-mat.str-el

Ferromagnetic Resonance Spectroscopy on the Kagome Magnet MgMn$_6$Sn$_6$

MgMn$_6$Sn$_6$ is the itinerant ferromagnet on the kagome lattice with high ordering temperature featuring complex electronic properties due to the nontrivial topological electronic band structure, where the spin-orbit coupling (SOC) plays a crucial role. Here, we report a detailed ferromagnetic resonance (FMR) spectroscopic study of MgMn$_6$Sn$_6$ aimed to elucidate and quantify the intrinsic magnetocrystalline anisotropy that is responsible for the alignment of the Mn magnetic moments in the kagome plane. By analyzing the frequency, magnetic field, and temperature dependences of the FMR modes, we have quantified the magnetocrystalline anisotropy energy density that reaches the value of approximately $ 3.5\cdot 10^6$ erg/cm$^3$ at $T = 3$ K and reduces to about $1\cdot 10^6$ erg/cm$^3$ at $T = 300$ K. The revealed significantly strong magnetic anisotropy suggests a sizable contribution of the orbital magnetic moment to the spin magnetic moment of Mn, supporting the scenario of the essential role of SOC for the nontrivial electronic properties of MgMn$_6$Sn$_6$.

cond-mat.str-el

Electron Spin Resonance Spectroscopy on Magnetic Van der Waals Compounds

The field of research on magnetic van der Waals compounds -- a special subclass of quasi-two-dimensional materials -- is currently rapidly expanding due to the relevance of these compounds to fundamental research where they serve as a playground for the investigation of different models of quantum magnetism and also in view of their unique magneto-electronic and magneto-optical properties pertinent to novel technological applications. The Electron Spin Resonance (ESR) spectroscopy plays an important role in the exploration of the rich magnetic behavior of van der Waals compounds due to its high sensitivity to magnetic anisotropies and unprecedentedly high energy resolution that altogether enable one to obtain thorough insights into the details of the spin structure in the magnetically ordered state and the low-energy spin dynamics in the ordered and paramagnetic phases. This article provides an overview of the recent achievements in this field made by the ESR spectroscopic techniques encompassing representatives of antiferro- and ferromagnetic van der Waals compounds of different crystal structures and chemical composition as well as of a special category of these materials termed magnetic topological insulators.

cond-mat.str-el

Phononic-magnetic dichotomy of the thermal Hall effect in the Kitaev-Heisenberg candidate material Na$_2$Co$_2$TeO$_6$

Majorana fermions as emergent excitations of the Kitaev quantum spin liquid ground state constitute a promising concept in fault tolerant quantum computation. Experimentally, the recently reported topological half-quantized thermal Hall effect in the Kitaev material $α$-RuCl$_3$ seems to confirm the Majorana nature of the material's magnetic excitations. It has been argued, however, that the thermal Hall signal in $α$-RuCl$_3$ rather stems from phonons or topological magnons than from Majorana fermions. Here we investigate the thermal Hall effect of the closely related Kitaev quantum material Na$_2$Co$_2$TeO$_6$, and we show that the thermal Hall signal emerges from at least two components, phonons and magnetic excitations. This dichotomy results from our discovery that the transversal heat conductivity $κ_{xy}$ carries clear signatures of the phononic $κ_{xx}$, but changes sign upon entering the low-temperature, magnetically ordered phase. We systematically resolve the two components by considering the detailed temperature and field dependence of both $κ_{xy}$ and $κ_{xx}$. Our results demonstrate that uncovering a genuinely quantized magnetic thermal Hall effect in a Kitaev topological quantum spin liquid requires to disentangle phonon vs. magnetic contributions where the latter include potentially fractionalized excitations such as the expected Majorana fermions.

cond-mat.str-el

Magnetic resonance study of rare-earth titanates

We present a nuclear magnetic resonance (NMR) and electron spin resonance (ESR) study of rare-earth titanates derived from the spin-1/2 Mott insulator YTiO$_3$. Measurements of single-crystalline samples of (Y,Ca,La)TiO$_3$ in a wide range of isovalent substitution (La) and hole doping (Ca) reveal several unusual features in the paramagnetic state of these materials. $^{89}$Y NMR demonstrates a clear discrepancy between the static and dynamic local magnetic susceptibilities, with deviations from Curie-Weiss behavior far above the Curie temperature $T_C$. No significant changes are observed close to $T_C$, but a suppression of fluctuations is detected in the NMR spin-lattice relaxation time at temperatures of about $3\times T_C$. Additionally, the nuclear spin-spin relaxation rate shows an unusual peak in dependence on temperature for all samples. ESR of the unpaired Ti electron shows broad resonance lines at all temperatures and substitution/doping levels, which we find to be caused by short electronic spin-lattice relaxation times. We model the relaxation as an Orbach process that involves a low-lying electronic excited state, which enables the determination of the excited-state gap from the temperature dependence of the ESR linewidths. We ascribe the small gap to Jahn-Teller splitting of the two lower Ti $t_{2g}$ orbitals. The value of the gap closely follows $T_C$ and is consistent with the temperatures at which deviations from Curie-Weiss fluctuations are observed in NMR. These results provide insight into the interplay between orbital and spin degrees of freedom in rare-earth titanates and indicate that full orbital degeneracy lifting is associated with ferromagnetic order.

cond-mat.str-el

Topological electronic structure and intrinsic magnetization in MnBi$_4$Te$_7$: a Bi$_2$Te$_3$-derivative with a periodic Mn sublattice

Combinations of non-trivial band topology and long-range magnetic order hold promise for realizations of novel spintronic phenomena, such as the quantum anomalous Hall effect and the topological magnetoelectric effect. Following theoretical advances material candidates are emerging. Yet, a compound with a band-inverted electronic structure and an intrinsic net magnetization remains unrealized. MnBi$_2$Te$_4$ is a candidate for the first antiferromagnetic topological insulator and the progenitor of a modular (Bi$_2$Te$_3$)$_n$(MnBi$_2$Te$_4$) series. For $n$ = 1, we confirm a non-stoichiometric composition proximate to MnBi$_4$Te$_7$ and establish an antiferromagnetic state below 13 K followed by a state with net magnetization and ferromagnetic-like hysteresis below 5 K. Angle-resolved photoemission experiments and density-functional calculations reveal a topological surface state on the MnBi$_4$Te$_7$(0001) surface, analogous to the non-magnetic parent compound Bi$_2$Te$_3$. Our results render MnBi$_4$Te$_7$ as a band-inverted material with an intrinsic net magnetization and a complex magnetic phase diagram providing a versatile platform for the realization of different topological phases.

cond-mat.mtrl-sci

Prediction and observation of the first antiferromagnetic topological insulator

Magnetic topological insulators (MTIs) are narrow gap semiconductor materials that combine non-trivial band topology and magnetic order. Unlike their nonmagnetic counterparts, MTIs may have some of the surfaces gapped due to breaking the time-reversal symmetry, which enables a number of exotic phenomena having potential applications in spintronics. So far, MTIs have only been created by means of doping nonmagnetic TIs with 3d transition metal elements, however, such an approach leads to strongly inhomogeneous magnetic and electronic properties of these materials, restricting the observation of important effects to very low temperatures. Finding intrinsic MTI, i.e. a stoichiometric well-ordered magnetic compound, could be an ideal solution to these problems, but no such material was observed to date. Here, using density functional theory we predict and further confirm by means of structural, transport, magnetic, angle- and spin-resolved photoemission spectroscopy measurements the realization of the antiferromagnetic (AFM) TI phase, that is hosted by the van der Waals layered compound MnBi$_2$Te$_4$. An interlayer AFM ordering makes MnBi$_2$Te$_4$ invariant with respect to the combination of the time-reversal ($\Theta$) and primitive-lattice translation ($T_{1/2}$) symmetries, $S = \Theta T_{1/2}$, giving rise to the $Z_2$ topological classification of AFM insulators. We find $Z_2 = 1$ for MnBi$_2$Te$_4$, which confirms its topologically nontrivial nature. The $S$-breaking (0001) surface of MnBi$_2$Te$_4$ exhibits a giant bandgap in the topological surface state as evidenced by ab initio calculations and photoemission measurements. These results culminate almost a decade-long search of an AFMTI, predicted in 2010. Furthermore, MnBi$_2$Te$_4$ is the first intrinsic magnetic TI realized experimentally.

cond-mat.mtrl-sci

Rolled-up self-assembly of compact magnetic inductors, transformers and resonators

Three-dimensional self-assembly of lithographically patterned ultrathin films opens a path to manufacture microelectronic architectures with functionalities and integration schemes not accessible by conventional two-dimensional technologies. Among other microelectronic components, inductances, transformers, antennas and resonators often rely on three-dimensional configurations and interactions with electromagnetic fields requiring exponential fabrication efforts when downscaled to the micrometer range. Here, the controlled self-assembly of functional structures is demonstrated. By rolling-up ultrathin films into cylindrically shaped microelectronic devices we realized electromagnetic resonators, inductive and mutually coupled coils. Electrical performance of these devices is improved purely by transformation of a planar into a cylindrical geometry. This is accompanied by an overall downscaling of the device footprint area by more than 50 times. Application of compact self-assembled microstructures has significant impact on electronics, reducing size, fabrication efforts, and offering a wealth of new features in devices by 3D shaping.

physics.app-ph

Probing the degree of spin polarization of a ferromagnet with ferromagnet/superconductor proximity effect

Superconductor/ferromagnet proximity effect has been studied for Pb/Co$_2$Cr$_{1-x}$Fe$_x$Al bilayers. Different substrate temperatures allowed us to prepare the Heusler alloy Co$_2$Cr$_{1-x}$Fe$_x$Al films with different degree of spin polarization of conduction band of the Heusler layer. We obtain a strong correlation between the dependence of the superconducting transition temperature on the Pb-layer thickness at fixed thickness of the Heusler layer and the degree of spin polarization in the ferromagnetic layer.

cond-mat.supr-con

Orbital reconstruction in nonpolar tetravalent transition-metal oxide layers

A promising route to tailoring the electronic properties of quantum materials and devices rests on the idea of orbital engineering in multilayered oxide heterostructures. Here we show that the interplay of interlayer charge imbalance and ligand distortions provides a knob for tuning the sequence of electronic levels even in intrinsically stacked oxides. We resolve in this regard the $d$-level structure of layered Sr$_2$IrO$_4$ by electron spin resonance. While canonical ligand-field theory predicts $g_{\parallel}$-factors $\!<\!2$ for positive tetragonal distortions as present in Sr$_2$IrO$_4$, the experiment indicates $g_{\parallel}\!>\!2$. This implies that the iridium $d$ levels are inverted with respect to their normal ordering. State-of-the-art electronic-structure calculations confirm the level switching in Sr$_2$IrO$_4$, whereas we find them in Ba$_2$IrO$_4$ to be instead normally ordered. Given the nonpolar character of the metal-oxygen layers, our findings highlight the tetravalent transition-metal 214 oxides as ideal platforms to explore $d$-orbital reconstruction in the context of oxide electronics.

cond-mat.str-el

Structure and Properties of α-NaFeO2-type Ternary Sodium Iridates

The synthesis, structure, and elementary magnetic and electronic properties are reported for layered compounds of the type Na3-xMIr2O6 and Na3-xM2IrO6, where M is a transition metal from the 3d series (M=Zn, Cu, Ni, Co, Fe and Mn). The rhombohedral structures, in space group R-3m, were determined by refinement of neutron and synchrotron powder diffraction data. No clear evidence for long range 2:1 or 1:2 honeycomb-like M/Ir ordering was found in the neutron powder diffraction patterns except in the case of M = Zn, thus in general the compounds are best designated as sodium deficient α-NaFeO2-type phases with formulas Na1-xM1/3Ir2/3O2 or Na1-xM2/3Ir1/3O2. Synchrotron powder diffraction patterns indicate that several of the compounds likely have honeycomb in-plane metal-iridium ordering with disordered stacking of the layers. All the compounds are sodium deficient under our synthetic conditions and are black and insulating. Weiss constants derived from magnetic susceptibility measurements indicate that Na0.62Mn0.61Ir0.39O2, Na0.80Fe2/3Ir1/3O2, Na0.92Ni1/3Ir2/3O2, Na0.86Cu1/3Ir2/3O2, and Na0.89Zn1/3Ir2/3O2 display dominant antiferromagnetic interactions. For Na0.90Co1/3Ir2/3O2 the dominant magnetic interactions at low temperature are ferromagnetic while at high temperatures they are antiferromagnetic; there is also a change in the effective moment. Low temperature specific heat measurements (to 2 K) on Na0.92Ni1/3Ir2/3O2 indicate the presence of a broad magnetic ordering transition. X-ray absorption spectroscopy shows that iridium is at or close to the 4+ oxidation state in all compounds. 23Na nuclear magnetic resonance measurements comparing Na2IrO3 to Na0.92Ni1/3Ir2/3O2 and Na0.89Zn1/3Ir2/3O2 provide strong indications that the electron spins are short-range ordered in the latter two materials. All of the compounds are spin glasses.

cond-mat.mtrl-sci

Interplay of Magnetic Exchange Interactions and Ni-S-Ni Bond Angles in Polynuclear Nickel(II) Complexes

The ability of bridging thiophenolate groups to transmit magnetic exchange interactions between paramagnetic Ni(II) ions has been examined. For this purpose, dinuclear and trinuclear Ni(II)-complexes were prepared and fully characterized by IR- and UV-vis spectroscopy, X-ray crystallography, static magnetization measurements and high-field electron spin resonance (HF-ESR). We compare structural and magnetic properties of the two Ni(II)-complexes and discuss the relationships between magnetic interactions and chemical bonding.

cond-mat.str-el